CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Xuechen Liu,Mingwen Wang,Shuai Yang,Xuexin Li,Kailai Lu,Yang Li,Juru Zhang,Jie Wu,Linghang Wang,Jinglei Li,Fei Li
Piezocatalysis presents an innovative catalytic technique that utilizes the piezoelectric properties of catalysts to convert mechanical energy into electrical energy, thereby driving chemical processes. While various methods for driving piezocatalytic reactions have been developed, there is a notable absence of comprehensive research on piezocatalytic performance across multiple methods. In this context, this study explores the potential of (1- x )Pb(Ni 1/3 Nb 2/3 )O 3 - x PbTiO 3 (PNN-PT) based catalysts as efficient piezocatalysts using both ultrasonic vibration and ball milling . The optimal reaction rate constants of the PNN-PT piezocatalyst under ultrasonic vibration and ball milling are found to be 0.0775 min −1 and 0.0265 min −1 , respectively. Notably, PNN-PT-based catalysts exhibit outstanding catalytic activity up to ultra-high substrate concentrations (65 mg/L), suggesting possible industrial applications. The exploration of the reaction mechanism indicates that •OH is the main reactive radical, the catalytic reaction activity demonstrates a direct relationship with •OH quenching, and the high •OH generation rate of PNN-PT further illustrated their suitability as environmental purification catalysts.
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ACS ES&T Engineering
·
2024
·
IF 7.4
Peijin Zou,Zhuangzhuang Ma,Zihuan Tang,Xiaotong Gao,Xiaoxiong Hou,Lichao Jia
Achieving the real-time detection of hydrogen sulfide (H2S) based on metal oxide semiconductor (MOS) gas sensors is of great significance for rapid disease diagnosis. However, the high-power consumption and poor selectivity severely limit its practice application. In this study, a platinum nanoparticle (Pt NPs)-loaded porous metal–organic framework (MOF)-derived SnO2 material was successfully synthesized to optimize the H2S-sensing performance at room temperature. The optimized Pt-loaded porous SnO2-based gas sensor exhibited remarkably high sensitivity (712–10 ppm), fast response (21 s), good selectivity, and extremely low detection limit for H2S (10 ppb) at room temperature. The in-depth analysis demonstrated that the porous structure of Sn-MOF can provide adequate active reaction sites for gas molecules. Moreover, the uniform distribution of surface-loaded Pt NPs can initiate electron and chemical sensitization effects, thereby improving the sensing performance. The successful application of Pt NPs provides a novel approach to improve the room-temperature (RT) sensing performance of metal-oxide-semiconductor-based gas sensors.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Kun Li,Chengjie Duan,Weitao Mao,Dongliang Wang,Yumeng Liang,Wenbo Ye,Guangke He,Xiang Liu
A direct and efficient synthesis of N-methyl-1,2,3,4-tetrahydroquinolines (MTHQs) is achieved through the one-pot reductive N-methylation of quinolines. The SnOx-decorated Pt/Al2O3 (Pt-SnOx/Al2O3) catalyst proves to be highly effective in the transformation from quinolines to MTHQs, using methanol as the exclusive source for hydrogen (H) and methyl (CH3), without the addition of additional bases or additives. Mechanistic and kinetic studies reveal a tandem reaction pathway: (1) the dehydrogenation of methanol, (2) reduction of quinolines to 1,2,3,4-tetrahydroquinolines (THQs), and (3) N-methylation of THQs to MTHQs, with the dehydrogenation of methanol identified as the rate-determining step. Characterization and catalytic performance results demonstrate that SnOx modifies the morphology and electronic properties of Pt-based metal active sites, which dramatically facilitates the cleavage of O–H and less reactive C–H bonds in methanol, and maintains a delicate balance between methanol dehydrogenation and reductive N-methylation of quinolines, thus obtaining a high reactivity for the total transformation.
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Journal of the American Chemical Society
·
2024
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IF 14.4
Baoxin Ni,Peng Shen,Guiru Zhang,Jiajun Zhao,Honghe Ding,Yifan Ye,Zhouying Yue,Hui Yang,Hao Wei,Kun Jiang
Pt is a well-known benchmark catalyst in the acidic oxygen reduction reaction (ORR) that drives electrochemical O2-to-H2O conversion with maximum chemical energy-to-electricity efficiency. Once dispersing bulk Pt into isolated single atoms, however, the preferential ORR pathway remains a long-standing controversy due to their complex local coordination environment and diverse site density over substrates. Herein, using a set of carbon nanotube supported Pt–N–C single-atom catalysts, we demonstrate how the neighboring N dopants regulate the electronic structure of the Pt central atom and thus steer the ORR selectivity; that is, the O2-to-H2O2 conversion selectivity can be tailored from 10% to 85% at 0.3 V versus reversible hydrogen electrode. Moreover, via a comprehensive X-ray-radiated spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy analysis coupled with theoretical modeling, we reveal that a dominant pyridinic- and pyrrolic-N coordination within the first shell of Pt–N–C motifs favors the 4e– ORR, whereas the introduction of a second-shell graphitic-N dopant weakens *OOH binding on neighboring Pt sites and gives rise to a dominant 2e– ORR. These findings underscore the importance of the chemical environment effect for steering the electrochemical performance of single-atom catalysts.
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BIOSENSORS & BIOELECTRONICS
·
2024
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IF 10.7
Yong Zhang,Zhihao Yang,Cailin Qiao,Yiyi Liu,Cuncun Wang,Xin Zeng,Jingzhou Hou,Danqun Huo,Changjun Hou
Real-time monitoring of biological markers in sweat is a valuable tool for health assessment. In this study, we have developed an innovative wearable biosensor for precise analysis of glucose in sweat during physical activities. The sensor is based on a single-atom catalyst of platinum (Pt) uniformly dispersed on tricobalt tetroxide (Co 3 O 4 ) nanorods and reduced graphene oxide (rGO), featuring a unique three-dimensional nanostructure and excellent glucose electrocatalytic performance with a wide detection range of 1-800 μM. Additionally, density functional theory calculations have revealed the synergetic role of Pt active sites in the Pt single-atom catalyst (Co 3 O 4 /rGO/Pt) in glucose adsorption and electron transfer, thereby enhancing sensor performance. To enable application in wearable devices, we designed an S-shaped microfluidic chip and a point-of-care testing (POCT) device, both of which were validated for effectiveness through actual use by volunteers. This research provides valuable insights and innovative approaches for analyzing sweat glucose using wearable devices, contributing to the advancement of personalized healthcare.
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Toxics
·
2025
·Vol. 13
·期 9
·737
·
IF 4.1
Wenqi He,Zhipeng Qie,Huaizhong Xiang,Hassan Alhassawi
Zeolites are promising materials for volatile organic compound (VOC) adsorption and catalytic oxidation, where tuning their structure via defect engineering can enhance adsorption capacity and active metal dispersion. In this study, a concentration-sensitive chelation strategy using diethylenetriaminepentaacetic acid (DTPA) was developed to achieve moderate dealumination for Beta and Y zeolites. For Y zeolite, 0.1 M DTPA treatment increased the toluene adsorption capacity from 59 to 110 mg/g. After platinum (Pt) loading, both DTPA-modified Beta- and Y-based catalysts showed improved toluene oxidation efficiency compared to their unmodified counterparts. Remarkably, the Y-DTPA-0.01-Pt catalyst achieved 90% toluene conversion at 150 °C with CO2selectivity above 90%. DRIFTS and H2-TPR results confirmed that moderate dealumination by DTPA generated silanol defects in zeolite Y that strongly anchored Pt2+in a highly dispersed form and suppressed PtO formation. Severe dealumination using 0.1 M DTPA created larger defects that favored the aggregation of Pt0clusters whilst causing significant loss in the micropores, thus reducing the Pt loading content and catalytic activity. This work demonstrates a simple and effective approach to optimize zeolite-based catalysts by controlling defect formation through controllable chelation, offering new insights into VOC abatement via tailored support design.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Baoqing Han,Song Xue,Benben Wang,Yuefei Yan,Hairong Wang,Congsi Wang
As a characteristic marker of advanced fibrosis, isoprene could be utilized for quick screening of liver disease. In this study, ZnO samples modified with varying molar percentages of Pt, as well as unmodified ZnO, were synthesized using hydrothermal method. The results revealed that the specific surface area (SSA) of the 1 mol% Pt@ZnO was as high as 51.6 m 2 /g and the original porous structure of ZnO was retained. The sensing performance of fabricated Pt@ZnO and ZnO was systematically evaluated, revealing enhanced isoprene detection capability for the 1 mol% Pt@ZnO compared to its unmodified counterpart. At an isoprene concentration of 0.2 ppm, the response time of Pt@ZnO was only 8 s, and the optimal temperature was lowered to 230 °C, facilitating rapid detection of isoprene with low power consumption. In addition, when exposed to 1 ppm isoprene, the 1 mol% Pt@ZnO exhibited a response value of 30.1, representing a threefold over pristine ZnO. Remarkably, the 1 mol% Pt@ZnO demonstrated remarkable sensitivity with a response value of 4.1 at 20 ppb isoprene concentration, while exhibiting superior selectivity towards isoprene compared to ZnO. In conclusion, 1 mol% Pt@ZnO spherical flower-like nanomaterial showed promise as candidate for isoprene gas-sensing applications.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Wang Xinzhong,Su Yiwen,Chen Jiashu,Yan Edward Hengzhou,Xia Qing,Wu Jie,Gong Shanhe,Tang Mingcong,Yip Wai Sze,Mu Yongbiao,Yi Yuyang,Wu Jinjin,Xu Fujing,Yang Xianzhong,Zhang Xiao,Dou Shixue,Sun Jingyu,Zheng Guangping
Current electrosynthesis catalysts typically rely on nanomaterial-based engineering with multi-dimensional structural modifications. However, such approaches may not always be necessary, especially for underexplored industrial electrochemical conversions. Here, we demonstrate that commercial platinum (Pt) foil catalysts excel in the electrochemical co-oxidation of waste polyethylene terephthalate (PET)-derived ethylene glycol (EG) and ammonia (NH 3 ) into formamide (HCONH 2 ), a process traditionally reliant on energy-intensive methods. This approach achieves a high Faradaic efficiency (FE) of 55.87 ± 1.4% and a productivity of 1003.63 ± 23.72 µmol cm −2 h −1 at industrially relevant current densities without any degradation for durable operation (more than 500 h and 300 h for H-cell and membrane electrode assembly (MEA) reactor, respectively). In situ spectroscopy, supported by theoretical calculations, suggests that *CH 2 O and *NH 2 are likely key intermediates. Furthermore, the product sustainability index (ProdSI) and techno-economic analysis (TEA) underscore the cost-effectiveness and sustainability of noble Pt foil in this scenario, challenging the conventional reliance on complex electrocatalysts. This work provides distinctive insights into catalyst screening and demonstrates a viable strategy for upcycling waste plastics.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yushun Wang,Xinzheng Zhang,Yuquan Yang,Huichao Wang,Woon-Ming Lau,Chenjing Wang,Zhongheng Fu,Dawei Pang,Qian Wang,Jinlong Zheng
The single atom catalysts (SACs) show immense promise as catalytic materials. By doping the single atoms (SAs) of precious metals onto substrates, the atomic utilization of these metals can be maximized, thereby reducing catalyst costs. The electronic structure of precious metal SAs is significantly influenced by compositions of doped substrates. Therefore, optimizing the electronic structure through appropriate doping of substrates can further enhance catalytic activity. Here, Pt single atoms (Pt SAs) are doped onto transition metal sulfide substrate NiS 2 (Pt SAs-NiS 2 ) and phosphide substrate Ni 2 P (Pt SAs-Ni 2 P) to design and prepare catalysts. Compared to the Pt SAs-NiS 2 catalyst, the Pt SAs-Ni 2 P catalyst exhibits better hydrogen evolution catalytic performance and stability. Under 1 M KOH conditions, the hydrogen evolution mass activity current density of the Pt SAs-Ni 2 P catalyst reaches 0.225 A mg Pt –1 at 50 mV, which is 33 times higher than that of commercial Pt/C catalysts. It requires only 44.9 mV to achieve a current density of 10 mA cm −2 . In contrast, for the Pt SAs-NiS 2 catalyst, the hydrogen evolution mass activity current density is 0.178 A mg Pt –1 , requiring 77.8 mV to achieve a current density of 10 mA cm −2 . Theoretical calculations indicate that in Pt SAs-Ni 2 P, the interaction between Pt SAs and the Ni 2 P substrate causes the Pt d-band center to shift downward, enhancing the H 2 O desorption and providing optimal H binding sites. Additionally, the hollow octahedral morphology of Ni 2 P provides a larger surface area, exposing more reactive sites and improving reaction kinetics. This study presents an effective pathway for preparing high-performance hydrogen evolution electrocatalysts by selecting appropriate doped substrates to control the electronic structure of Pt SAs.
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ACS Nano
·
2024
·
IF 15.8
Daoru Liu,Feifei Jiang,Qinghua Zhang,Wei-Hsiang Huang,Yanping Zheng,Mingshu Chen,Liming Wu,Ruixuan Qin,Mingzhi Wang,Shiyi Zhang,Limin Chen,Keyou Yan,Linan Zhou,Yun Zhao,Lin Gu,Guangxu Chen
Bimetallic Pt-based catalysts, for example, PtZn and PtSn catalysts, have gained significant attention for addressing the poor stability and low selectivity of pristine Pt catalysts over propane dehydrogenation (PDH). However, the structures of the active sites and the corresponding catalytic mechanism of PDH are still elusive. Here, we demonstrate a spatially confined Pt–ZnmOx@RUB-15 catalyst (where “m” is the mole ratio of Zn/Pt and RUB-15 is a layered silica), which exhibited high catalytic activity, ultrahigh selectivity (>99%), and resistance to coking at 550 °C for PDH. Significantly different from the preliminary studies over the PtZn catalysts, through the assistance of quasi-in situ X-ray photoelectron spectroscopy (XPS), in situ Fourier transform infrared spectroscopy (CO-FTIR), in situ X-ray absorption spectroscopy (XAS), and CO titration, we discovered that the active sites for PDH were the Pt–ZnOx interfaces, characterized by a structure of Ptδ+–Zn2+–O–Si. Density functional theory (DFT) calculations showed that Pt atoms positioned at Pt–ZnOx interfaces with coordinatively unsaturated ZnOx sites facilitate the C–H bond breaking of propane while concurrently suppressing deep dehydrogenation processes. This study suggests that engineering the interfaces of Pt–metal oxides under spatially confined conditions holds promise for developing highly efficient Pt-based catalysts for light alkane dehydrogenation.
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TALANTA
·
2024
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IF 5.6
Yanli Lei,Xinyan He,Yu Zeng,Xinyu Wang,Le Yang,Xiaowen Liu,Zhihe Qing
Gold nanoparticles (Au NPs) have been widely utilized in developing DNAzyme-functionalized nanosensors, most of which were engineered by attaching the thiolated DNAzymes to Au NPs via Au-S bonding. However, the Au NP-DNAzyme nanosensors always suffer from signal distortion when applied in complex environment with abundant thiols, which poses challenge for practical applications. Here, we focus on addressing the root cause of the issue and propose to decorate the Au NPs with a thin layer of platinum, thus facilitating the conjugation of DNAzymes through Pt-S bonding, a thiol-resistant cross-linking. The Pt-S bond stabilized DNAzyme nanosensor effectively minimized false positive signals when detecting L-histidine in infant formulas, as compared to the Au-S stabilized counterpart. This innovative strategy holds promise for high-fidelity biosensing, improving the practical applicability of Au NP-based DNAzyme nanosensor.
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Small
·
2024
·
IF 13
Yuxin Gao,Hang Liu,Xintian Wang,Xiao Liu,Bin Shan,Rong Chen
Pt-based alloy with high mass activity and durability is highly desired for proton exchange membrane fuel cells, yet a great challenge remains due to the high mass transport resistance near catalysts with lowering Pt loading. Herein, an extensible approach employing atomic layer deposition to accurately introduce a gas-phase metal precursor into platinum nanoparticles (NPs) pre-filled mesoporous channels is reported, achieved by controlling both the deposition site and quantity. Following the spatially confined alloying treatment, the prepared PtSn alloy catalyst within mesopores demonstrates a small size and homogeneous distribution (2.10 ± 0.53 nm). The membrane electrode assembly with mesoporous carbon-supported PtSn alloy catalyst achieves a high initial mass activity of 0.85 A mg Pt − 1 ${\mathrm{mg}}_{\mathrm{Pt}}^{-1}$ at 0.9 V, which is attributed to the smallest local oxygen transport resistance (3.68 S m −1 ) ever reported. The mass activity of the catalyst only decreases by 11% after 30000 cycles of accelerated durability test, representing superior full-cell durability among the reported Pt-based alloy catalysts. The enhanced activity and durability are attributed to the decreased adsorption energy of oxygen intermediates on Pt surface and the strong electronic interaction between Pt and Sn inhibiting Pt dissolution.
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